Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 117, Issue 48, Pages 12912-12921Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp408672m
Keywords
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Funding
- Ministry of Education, Culture, Sports, Science, and Technology in Japan [20120003]
- Japan Society for the Promotion of Science for young scientists
- Grants-in-Aid for Scientific Research [20120003] Funding Source: KAKEN
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Ethylene ozonolysis was investigated in laboratory experiments using a Teflon bag reactor. A negative ion chemical ionization mass spectrometer (NI-CIMS) using SO2Cl- and Cl- as reagent ions was used for product analysis. In addition to the expected gas-phase products, such as formic acid and hydroperoxymethyl formate, oligomeric hydroperoxides composed of the Criegee intermediate (CH2OO) as a chain unit were observed. Furthermore, we observed secondary organic aerosol (SOA) formation from the ethylene ozonolysis, and the particle-phase products were also analyzed by NI-CIMS. The CH2OO oligomers were also observed as particle-phase components, suggesting that the oligomeric hydroperoxides formed in the gas phase partition into the particle phase. By adding methanol as a stabilized Criegee intermediate scavenger, both the gas-phase oligomer formation and SOA formation were strongly suppressed. This indicates that CH2OO plays a critical role in the formation of oligomeric hydroperoxides followed by SOA formation in ethylene ozonolysis. A new formation mechanism for the oligomeric hydroperoxides, which includes sequential addition of CH2OO to hydroperoxides, is proposed.
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